Near Infrared-Activatable Methylene Blue Polypeptide Codelivery of the NO Prodrug via π–π Stacking for Cascade Reactive Oxygen Species Amplification-Mediated Photodynamic Therapy

前药 活性氧 光动力疗法 谷胱甘肽 生物物理学 光敏剂 纳米载体 化学 材料科学 光化学 生物化学 药物输送 纳米技术 生物 有机化学
作者
Yu Zhang,Peng Zhao,Xiaoai Chen,Chang Xu,Jingzhe Guo,Xiongwei Qu,Xiuli Hu,Hui Gao,Pingsheng Huang,Jimin Zhang
出处
期刊:ACS Applied Materials & Interfaces [American Chemical Society]
卷期号:15 (10): 12750-12765 被引量:17
标识
DOI:10.1021/acsami.2c21280
摘要

The application of photodynamic therapy (PDT) has attracted remarkable interest in cancer treatment because of the advantages of noninvasiveness and spatiotemporal selectivity. However, the PDT efficiency is considerably limited by photosensitizer (PS) quenching and severe hypoxia in solid tumors. Herein, a kind of near infrared (NIR)-activatable methylene blue (MB) peptide nanocarrier was developed for codelivery of nitric oxide (NO) prodrug JSK, expecting a cascade of reactive oxygen species (ROS) amplification-mediated antitumor PDT. In detail, MB was conjugated to water-soluble polyethylene glycol-polylysine (PEG-PLL) through NIR-photocleavable 10-N-carbamoyl bonds, and the subsequent amphiphilic conjugates (mPEG-PLL-MB) self-assembled into nanoparticles (NPs), which allowed JSK codelivery via π-π stacking interactions. MB in quenched state in mPEG-PLL-MB/JSK NPs could be photoactivated by NIR light locoregionally in a controlled manner due to the photocleavage of carbamoyl bonds. Apart from ROS production, assembly disturbance and even disintegration of mPEG-PLL-MB/JSK occurred along with MB activation that subsequently freed JSK, which was further triggered by intracellularly overexpressed glutathione (GSH) and glutathione S-transferase (GST) to sustain the release of NO. NO then served as a hypoxia relief agent through inhibition of cellular respiration to economize O2, cooperating with MB activation and GSH depletion, which synergistically enabled a cascade of ROS amplification to augment PDT for mitochondrial apoptosis-mediated tumor inhibition in vitro and in vivo. Therefore, this pioneering strategy of cascade amplification of ROS addressed the key issues of PS inactivation, hypoxia resistance, and ROS neutralization in a three-pronged approach, which hold great promise in efficient antitumor PDT.
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